日本冲绳科学技术大学院大学戚亚冰课题组---基于同轴CNTs@TiN-TiO2海绵的长寿命高面积容量的Li-S电池
异质结构的合理设计为锂硫电池中多硫化锂转化的理想催化剂体系开辟了新的机遇。但其传统的制作工艺复杂，难以合理控制各组分的含量和分布。在这项工作中，为了合理设计异质结构，利用原子层沉积（ALD）方法在通过化学气相沉积（CVD）制备的三维（3D）独立式碳纳米管（CNTs）骨架的基础上制备了同轴CNTs@TiN-TiO2海绵。通过控制CNT外表面的TiO2和TiN层的厚度，并结合退火后处理，由10 nm TiN和5 nm TiO2包裹的CNTs混合得到了同轴CNTs@TiN-TiO2海绵。通过测试发现，同轴CNTs@TiN-TiO2海绵表现出优异的性能，提高了Li-S电池的性能。其中，在0.2 C下具有1431 mAh g-1的高比容量，即使在1 C下也具有1289 mAh g-1的高比容量，在2 C下循环500次后容量保持率仍高达85%。此外，3D CNTs海绵的多孔结构和相互连接的导电通路有助于容纳大量S并保证其有效的利用。结果表明，基于同轴CNTs@TiN-TiO2海绵的Li-S电池的面容量高达21.5 mAh cm-2，远高于商用锂离子电池（LIBs）的面容量（4 mAh cm-2），并且与最近报道的S载量高于8 mg cm-2 的Li-S电池系统相当。该策略还可以扩展到其他同轴/逐层异质结构的优化，并促进形成连续且匹配良好的界面，在储能和催化方面具有广阔的应用前景。
Figure 1. CNTs@TiN-TiO2的制备及多硫化物转化过程示意图
Figure 2. CNTs@TiN-TiO2-5的形貌表征。（a）CNTs@TiN-TiO2-5的TEM图，显示了涂覆在CNT表面上的集成TiN-TiO2异质结构；（b）CNTs@TiN-TiO2-5的TEM图及其C、O、N和Ti的相应元素映射，显示了TiN-TiO2异质结构的混合均匀分布。（c）CNTs@TiN-TiO2-5的高分辨率TEM图，显示了TiN-TiO2异质结构的良好匹配界面。
Figure 3 . CNTs@TiN-TiO2-5的多硫化锂吸附测试和相应的XPS表征。（a）将杂化物浸入Li2S6溶液（0.005 M）中，比较CNTs@TiN-TiO2-2、CNTs@TiN-TiO2-5和CNTs@TiN-TiO2-10的多硫化物吸附能力；（b-c）CNTs@TiN-TiO2-5中Ti 2p和N 1s在多硫化物吸附前后的XPS光谱。
Figure 4. 恒电位放电条件下的Li2S沉积过程。（a）CNTs@TiN-TiO2-2，（b）CNTs@TiN-TiO2-5，（c）CNTs@TiN-TiO2-10在2.05 V下的恒电位放电曲线。
Figure 5. CNTs@TiN-TiO2-2、CNTs@TiN-TiO2-5、CNTs@TiN-TiO2-10的电化学性能。（a）在扫描速率为0.1 mV s-1时的CV曲线，（b）恒电流充电和放电曲线，（c）EIS曲线；（d）CNTs@TiN-TiO2-5、CNTs@TiN-TiO2-2和CNTs@TiN-TiO2-10在0.1-5 C时的倍率性能。
Figure 6. CNTs@TiN-TiO2-2、CNTs@TiN-TiO2-5、CNTs@TiN-TiO2-10的循环性能。（a）CNTs@TiN-TiO2-5、CNTs@TiN-TiO2-2和CNTs@TiN-TiO2-10在0.2 C下循环100次后的循环稳定性比较；（b）CNTs@TiN-TiO2-5在1 C下的长期循环性能。
相关研究成果由日本冲绳科学技术大学院大学Yabing Qi课题组于2021年发表在《Nature Communications》（https://doi.org/10.1038/s41467-021-24976-y）上。原文：Long-life lithium-sulfur batteries with high areal capacity based on coaxial CNTs@TiN-TiO2 sponge。
戚亚冰Yabing Qi
FRSC, Professor
Energy Materials and Surface Sciences Unit (EMSSU)
Okinawa Institute of Science and Technology Graduate School (OIST)
1919-1 Tancha, Onna-son, Kunigami-gun
Okinawa, Japan 904-0412 (E-Mail: Yabing.Qi at OIST.jp)
Education
PhD (UC Berkeley, 2008).
MPhil (Hong Kong University of Science and Technology, 2002).
BSc (Nanjing University, 2000).
Nationality
China
Selected Publications and Patent Applications (Link)
Google Scholar Citations
Invited Journal Referee for
Science, Science Advances, Nature, Nature Communications, Nature Energy, Nature Photonics, Nature Materials, Nature Nanotechnology, Physical Review Letters, Journal of the American Chemical Society, Angewandte Chemie International Edition, Advanced Materials, Energy & Environmental Science, Nano Letters, ACS Nano, Chemistry of Materials, ACS Energy Letters, The Journal of Physical Chemistry Letters, Applied Physics Letters, Advanced Materials Interfaces, Langmuir, Physical Chemistry Chemical Physics, Advanced Energy Materials, Advanced Functional Materials, Physical Review B, Physical Review E, Nanotechnology, Organic Electronics, Applied Surface Science, CrystEngComm, etc.
Organizing of Conferences and Symposia
Symposium Chair
International Symposium on Organic Electronics
OIST, Okinawa, Japan
October 3 - 5, 2012.
Symposium Chair
International Symposium on Functional Materials
OIST, Okinawa, Japan
January 25 - 29, 2016.
Symposium Co-organizer
2016 MRS Fall Meeting - Symposium ES3, “Perovskite Solar Cell Research from Material Properties to Photovoltaic Function.” (Call for Papers)
Boston, Massachusetts, USA
November 27 - December 2, 2016.
Symposium Lead Organizer
2017 MRS Spring Meeting - Symposium ES1, “Perovskite Solar Cells—Towards Commercialization” (Call for Papers)
Phoenix, Arizona, USA
April 17 - 21, 2017.
Symposium Lead Organizer
2017 MRS Fall Meeting - Symposium ES1, “Perovskite Materials and Devices—Progress and Challenges” (Call for Papers)
Boston, Massachusetts, USA
November 26 - December 1, 2017.
Symposium Chair
International Symposium on Energy Science and Technology
OIST, Okinawa, Japan
January 22 - 26, 2018.
Symposium Lead Organizer
2018 MRS Spring Meeting - Symposium EN02, “Advances in Perovskite Solar Cell Devices and Applications” (Call for Papers)
Phoenix, Arizona, USA
April 2 - 6, 2018.
Symposium Co-organizer
2018 MRS Spring Meeting - Symposium ES15, “Fundamental Understanding of the Multifaceted Optoelectronic Properties of Halide Perovskites” (Call for Papers)
Phoenix, Arizona, USA
April 22 - 26, 2019.
Symposium Co-organizer
2019 MRS Fall Meeting - Symposium EN08, “Halide Perovskites for Photovoltaic Applications—Devices, Stability and Upscaling” (Call for Papers)
Boston, Massachusetts, USA
December 1 - 6, 2019.
Symposium Chair
International Symposium on Sustainable Energy and Development (Call for Poster Presentation Participants)
OIST, Okinawa, Japan
Febuary 24 - 28, 2020.